The field of semiconductor nanowires (NWs) has become one of the most active and mature research areas. However, progress in this field has been limited, due to the difficulty in controlling the density, orientation, and placement of the individual NWs, parameters important for mass producing nanodevices. The work presented herein describes a novel nanosynthesis strategy for ultrathin self-aligned silicon carbide (SiC) NW arrays (≤ 20 nm width, 130 nm height and 200–600 nm variable periodicity), with high quality (~2 Å surface roughness, ~2.4 eV optical bandgap) and reproducibility at predetermined locations, using fabrication protocols compatible with silicon microelectronics. Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, ultraviolet-visible spectroscopic ellipsometry, atomic force microscopy, X-ray diffractometry, and transmission electron microscopy studies show nanosynthesis of high-quality polycrystalline cubic 3C-SiC materials (average 5 nm grain size) with tailored properties. An extension of the nanofabrication process is presented for integrating technologically important erbium ions as emission centers at telecom C-band wavelengths. This integration allows for deterministic positioning of the ions and engineering of the ions’ spontaneous emission properties through the resulting NW-based photonic structures, both of which are critical to practical device fabrication for quantum information applications. This holistic approach can enable the development of new scalable SiC nanostructured materials for use in a plethora of emerging applications, such as NW-based sensing, single-photon sources, quantum LEDs, and quantum photonics.